Defective SiC nanotube based single-atom catalysts for electrocatalytic nitrogen fixation with curvature effect

被引:3
作者
Wang, Zhiwei [1 ]
Gao, Shuaishuai [1 ]
Liu, Xiaojing [1 ]
Chen, Xin [2 ]
Zhang, Xintao [1 ]
Sa, Rongjian [3 ]
Li, Qiaohong [4 ]
Sun, Chenghua [5 ]
Ma, Zuju [1 ]
机构
[1] Yantai Univ, Sch Environm & Mat Engn, Yantai 264005, Peoples R China
[2] Yantai Univ, Sch Comp & Control Engn, Yantai 264005, Peoples R China
[3] Minjiang Univ, Coll Mat & Chem Engn, Fuzhou 350108, Peoples R China
[4] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
[5] Swinburne Univ Technol, Fac Sci Engn & Technol, Dept Chem & Biotechnol, Hawthorn, Vic 3122, Australia
来源
MOLECULAR CATALYSIS | 2023年 / 549卷
基金
美国国家科学基金会;
关键词
Nitrogen reduction; Single-atom catalysts; Curvature effect; Density functional theory; Nanotube; SILICON-CARBIDE NANOTUBES; REDUCTION REACTION; THEORETICAL EVALUATION; METALLOPORPHYRIN MP; EVOLUTION REACTION; AMMONIA-SYNTHESIS; N-2; FIXATION; CARBON; FE; CO;
D O I
10.1016/j.mcat.2023.113519
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The production of fertilizers, explosives, and various other chemicals relies heavily on ammonia (NH3). Electrochemical reduction of nitrogen to ammonia, also known as the nitrogen reduction reaction (NRR), is a potential alternative to the Haber-Bosch process that can be carried out at ambient conditions. However, many NRR catalysts suffer from low selectivity and require a large overpotential to drive the reaction, limiting their practical application. In this study, we used density functional theory (DFT) calculations to investigate the mechanistic aspects of the NRR and the effect of curvature variation on the catalytic activity of silicon carbide nanotubes (SiCNTs) decorated with 3d-5d transition metal single-atom catalysts. Our results suggest that the Os@SiCNT catalyst exhibits promising activity as an eNRR catalyst with an overpotential of 0.47 V and high selectivity over hydrogen evolution reaction (HER) competition. The electronic "acceptance-donation" interaction between N2 and Os promotes the adsorption and activation of N2 molecules on the catalyst surface. Additionally, our findings demonstrate that as the nanotube diameter decreases, the energy barrier for the NRR reaction decreases as well. However, this decrease in diameter also leads to a weaker capacity for *N2 adsorption, which may ultimately reduce the selectivity of the NRR reaction. These findings offer valuable insights that can aid in the rational design of nanotube-based electrocatalysts for eNRR.
引用
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页数:8
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